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A Dynamic Metal-Organic Radical Emission System

Angewandte Chemie 2024年第12期137卷

作者： Xiang Li Prof. Yuan Wang Prof. Glib V. Baryshnikov Ihor Sahalianov Prof. Hans Ågren Yuri Tanuma Prof. Zhiyun Zhang Prof. Cheng Qian Dr. Muyu Cong Prof. Tao Yi Prof. Hongwei Wu State Key Laboratory for Modification of Chemical Fiber and Polymer Materials Key Lab of Science and Technology of Eco-Textile Ministry of Education College of Chemistry and Chemical Engineering Donghua University Shanghai 201620 China Beijing National Laboratory of Molecular Sciences and CAS Key Laboratory of Colloid Interface and Thermodynamics Institute of Chemistry Chinese Academy of Sciences North First Street 2 Zhongguancun Beijing 100190 China Laboratory of Organic Electronics Department of Science and Technology Linköping University SE-60174 Norrköping Sweden Wallenberg Initiative Materials Science for Sustainability Department of Science and Technology Linköping University SE-60174 Norrköping Sweden Department of Physics and Astronomy Uppsala University Uppsala SE-751 20 Sweden Jožef Stefan Institute Jamova 39 1000 Ljubljana Slovenia Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Center for Materiobiology and Dynamic Chemistry East China University of Science & Technology Shanghai 200237 P. R. China

Developing new organic radical emission systems and regulating their luminescence properties presents a significant challenge. Herein, we build dynamic and multi-emission band radical luminescence systems by co-assembling inorganic metal salts with carbonyl compounds in ionic liquids. After the assembling, dual-band, and excitation wavelength-dependent emission was observed upon ultraviolet light irradiation, one emission band originates from carbonyl radical after light irradiation, the other band from the ligand-metal charge transfer (LMCT) state, which benefits from the charge transfer from the radicals to the metal salts. The dual emission centers also introduce excitation wavelength-dependent properties for the molecules. In addition, three-band emission covering the visible and near-infrared regions can be shown when two or three kinds of metal ions are simultaneously doped into the radical system driven by the ligand-metal-metal charge transfer (LMMCT). Interestingly, visible light can quickly quench the radical emission of systems, thus realizing a dynamic luminescence. The LMMCT effect and strong supramolecular interactions significantly improve the photoluminescence quantum yield by up to 67.2 %. Moreover, such materials can be successfully used for detecting radioactive metal ions and information encryption. This study develops a platform for manufacturing various metal-organic radical emission systems with diverse properties.

关键词： metal-organic radical multi-band emission dynamic luminescence supramolecular interactions information encryption

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Ambient Chemical Fixation of CO2 Using a Robust Ag27 Cluster-Based Two-Dimensional Metal–Organic Framework

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Angewandte Chemie 2020年第45期132卷

作者： Zhao M. Huang S. Fu Q. Li W. Guo R. Yao Q. Wang F. Cui P. Tung C.-H. Sun D. School of Chemistry and Chemical Engineering Key Lab of Colloid and Interface Chemistry of Ministry of Education State Key Laboratory of Crystal Materials Shandong University Jinan 250100 China School of Physics Shandong University Jinan 250100 China School of Chemistry and Chemical Engineering Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology Liaocheng University Liaocheng 252000 China School of Materials Science and Engineering Shandong University Jinan 250061 China Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University Tianjin 300071 China College of Chemistry Chemical Engineering and Materials Science Shandong Provincial Key Laboratory of Clean Production of Fine Chemicals Shandong Normal University Jinan 250014 China

Unprecedented double S2− templated Ag27 clusters have been stabilized by 5,10,15,20-tetra(4-pyridyl)porphyrin (TPyP-H2) ligands to afford a robust 2D metal–organic framework (Ag27-MOF). This silver cluster-assembled material serves as a highly efficient heterogeneous catalyst for the cyclization of both terminal and internal propargylamines with CO2 under atmospheric pressure. Density functional theory (DFT) calculations illustrate that the high catalytic activity and broad substrate scope are attributable to the saddle-shaped metallic node in Ag27-MOF, which features an accessible platform with high-density silver atoms as π-Lewis acid sites for activating C≡C triple bonds. As a result, different sterically hindered alkyne substrates can be effectively activated through π-interactions with these cationic silver centers. © 2020 Wiley-VCH GmbH

关键词： 2D metal–organic frameworks CO2 fixation heterogeneous catalysis silver cluster-assembled materials

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Dynamic chloride ion adsorption on single iridium atom boosts seawater oxidation catalysis

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Nature communications 2024年第1期15卷 1973页

作者： Xinxuan Duan Qihao Sha Pengsong Li Tianshui Li Guotao Yang Wei Liu Ende Yu Daojin Zhou Jinjie Fang Wenxing Chen Yizhen Chen Lirong Zheng Jiangwen Liao Zeyu Wang Yaping Li Hongbin Yang Guoxin Zhang Zhongbin Zhuang Sung-Fu Hung Changfei Jing Jun Luo Lu Bai Juncai Dong Hai Xiao Wen Liu Yun Kuang Bin Liu Xiaoming Sun State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering College of Chemistry Beijing University of Chemical Technology Beijing 100029 PR China. School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University Singapore 637459 Singapore. Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid Interface and Chemical Thermodynamics Institute of Chemistry Chinese Academy of Sciences Beijing 100190 PR China. Ocean Hydrogen Energy R&D Center Research Institute of Tsinghua University in Shenzhen Shenzhen 518057 PR China. State Key Lab of Organic-Inorganic Composites College of Chemical Engineering Beijing University of Chemical Technology 100029 Beijing PR China. Energy & Catalysis Center School of Materials Science & Engineering Beijing Institute of Technology Beijing 100081 PR China. Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei 230026 PR China. Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences 100049 Beijing PR China. Department of Chemistry Tsinghua University 100084 Beijing PR China. Department of Materials Science and Engineering City University of Hong Kong Hong Kong SAR 999077 PR China. College of Energy Shandong University of Science and Technology Tsingtao 266590 PR China. Beijing Key Laboratory of Energy Environmental Catalysis Beijing University of Chemical Technology 100029 Beijing PR China. Department of Applied Chemistry and Center for Emergent Functional Matter Science National Yang Ming Chiao Tung University Hsinchu 300 Taiwan. School of Materials Science and Engineering Tianjin Key Lab of Photoelectric Materials & Devices Tianjin University of Technology Tianjin 300384 PR China. ShenSi Lab Shenzhen Institute for Advanced Study University of Electronic Science and Technology of China Shen

Seawater electrolysis offers a renewable, scalab.e, and economic means for green hydrogen production. However, anode corrosion by Cl pose great challenges for its commercialization. Herein, different from conventional catalysts designed to repel Cl adsorption, we develop an atomic Ir catalyst on cobalt iron layered double hydroxide (Ir/CoFe-LDH) to tailor Cl adsorption and modulate the electronic structure of the Ir active center, thereby establishing a unique Ir-OH/Cl coordination for alkaline seawater electrolysis. Operando characterizations and theoretical calculations unveil the pivotal role of this coordination state to lower OER activation energy by a factor of 1.93. The Ir/CoFe-LDH exhibits a remarkable oxygen evolution reaction activity (202 mV overpotential and TOF = 7.46 O s) in 6 M NaOH+2.8 M NaCl, superior over Cl-free 6 M NaOH electrolyte (236 mV overpotential and TOF = 1.05 O s), with 100% catalytic selectivity and stability at high current densities (400-800 mA cm) for more than 1,000 h.

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Author Correction: Moiré two-dimensional covalent organic framework superlattices

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Nature chemistry 2025年 2025 May 21页

作者： Gaolei Zhan Brecht Koek Yijia Yuan Yikuan Liu Vipin Mishra Veniero Lenzi Karol Strutyński Chunxiao Li Rongrong Zhang Xin Zhou Hwa Seob Choi Zhen-Feng Cai Joaquín Almarza Kunal S Mali Aurelio Mateo-Alonso Manuel Melle Franco Yihan Zhu Steven De Feyter Kian Ping Loh Department of Chemistry National University of Singapore Singapore Singapore. gaolei.zhan2022@***. i-Lab Nano-X Vacuum Interconnected Workstation Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO) Chinese Academy of Sciences (CAS) Suzhou P. R. China. gaolei.zhan2022@***. Department of Chemistry Division of Molecular Imaging and Photonics KU Leuven Leuven Belgium. Department of Chemistry National University of Singapore Singapore Singapore. Center for Electron Microscopy Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts China-Saudi Arabia Joint Laboratory on Microscopic Structural Engineering of Advanced Materials and College of Chemical Engineering Zhejiang University of Technology Hangzhou P. R. China. CICECO-Aveiro Institute of Materials Department of Chemistry University of Aveiro Aveiro Portugal. i-Lab Nano-X Vacuum Interconnected Workstation Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO) Chinese Academy of Sciences (CAS) Suzhou P. R. China. Key Laboratory of Green Chemistry and Technology of Ministry of Education College of Chemistry Sichuan University Chengdu P. R. China. POLYMAT University of the Basque Country UPV/EHU Donostia-San Sebastian Spain. Ikerbasque Basque Foundation for Science Bilbao Spain. Center for Electron Microscopy Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts China-Saudi Arabia Joint Laboratory on Microscopic Structural Engineering of Advanced Materials and College of Chemical Engineering Zhejiang University of Technology Hangzhou P. R. China. yihanzhu@***. Department of Chemistry Division of Molecular Imaging and Photonics KU Leuven Leuven Belgium. steven.defeyter@kuleuven.be. Department of Chemistry National University of Singapore Singapore Singapore. chmlohkp@nus.edu.sg.

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Unexpected Stacking Transformation from H- To J- To X-Aggregated Co-Crystals Leading to Tunable Mechanical and Optoelectronic Properties

SSRN

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SSRN 2020年

作者： Ji, Wei Xue, Bin Bera, Santu Guerin, Sarah Liu, Yanqing Yuan, Hui Li, Qi Yuan, Chengqian Shimon, Linda J.W. Ma, Qing Kiely, Evan Tofail, Syed A.M. Si, Mingsu Yan, Xuehai Cao, Yi Wang, Wei Yang, Rusen Thompson, Damien Li, Junbai Gazit, Ehud School of Molecular Cell Biology and Biotechnology George S. Wise Faculty of Life Sciences Tel Aviv University Tel Aviv6997801 Israel National Laboratory of Solid State Microstructure Department of Physics Nanjing University NanjingJiangsu210093 China Department of Physics Bernal Institute University of Limerick V94 T9PX Ireland Key Laboratory for Magnetism and Magnetic Materials of the Ministry of Education Lanzhou University Lanzhou730000 China Beijing National Laboratory for Molecular Sciences CAS Key Lab of Colloid Interface and Chemical Thermodynamics Institute of Chemistry Chinese Academy of Sciences Beijing100190 China School of Advanced Materials and Nanotechnology Xidian University Xi’an710126 China State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Department of Chemical Research Support Weizmann Institute of Science Rehovot76100 Israel Institute of Chemical Materials China Academy of Engineering Physics Mianyang621900 China Department of Materials Science and Engineering Iby and Aladar Fleischman Faculty of Engineering Tel Aviv University Tel Aviv6997801 Israel

Molecular stacking modes, generally classified as H-, J-, and X-aggregation play a key role in determining the optoelectronic properties of organic crystals. However, the control of stacking transitions of a specific molecule is an unmet challenge and a priori prediction of performance in different stacking modes is currently not possible. Herein, unexpected stacking transition from H- to J- and X- aggregation is observed in the crystal structure of a minimalistic aromatic molecule, 4,4’-bipyridine, upon co-assembled with N-acetyl-L-alanine, a non-aromatic amino acid derivative. This stacking transition improves the physicochemical properties of the co-crystals, including a large red-shifted emission, enhanced chirality, improved thermal stability and mechanical properties. While the single crystal of 4,4’-Bpy shows good optical waveguiding and piezoelectric properties, the co-crystal has a significantly lower band-gap and improved conductivity. This demonstrates the first example of H- to J- and X- packing transition of a minimalistic model by co-crystal aggregation and provides a proof-of-concept strategy for organic optoelectronics design. © 2020, The Authors. All rights reserved.

关键词： Supramolecular chemistry

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Nanodevices: Record‐Low‐Threshold Lasers Based on Atomically Smooth Triangular Nanoplatelet Perovskite (Adv. Funct. Mater. 2/2019)

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advanced Functional materials 2019年第2期29卷

作者： Guohui Li Tao Che Xingqi Ji Shaoding Liu Yuying Hao Yanxia Cui Shengzhong Liu Key Lab of Advanced Transducers and Intelligent Control System of Ministry of Education College of Physics and Optoelectronics Key Laboratory of Interface Science and Engineering in Advanced Materials Taiyuan University of Technology Taiyuan 030024 P. R. China State Key Laboratory of Quantum Optics and Quantum Optics Devices Shanxi University Taiyuan 030006 P. R. China Key Laboratory of Applied Surface and Colloid Chemistry National Ministry of Education Shaanxi Engineering Lab for Advanced Energy Technology School of Materials Science and Engineering Shaanxi Normal University Xi'an 710119 P. R. China

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Anomalously enhanced thermal stability of phosphorene via metal adatom doping: An experimental and first-principles study

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Nano Research 2016年第9期9卷 2687-2695页

作者： Xuewei Feng Vadym V.Kulish Ping Wu xinke Liu Kah-Wee Ang Department of Electrical and Computer Engineering National University of Singapore4 Engineering Drive 3Singapore 117583Singapore Entropic Interface Group(EIG) Engineering Product DevelopmentSingapore University of Technology and Design(SUTD)8 Somapah RoadSingapore 487372Singapore College of Materials Science and Engineering Shenzhen Engineering Laboratory for Advanced Technology of CeramicsNanshan District Key Lab for Biopolymer and Safety EvaluationShenzhen University3688 Nanhai AvenueShenzhen 518060China

Atomically thin black phosphorus, also known as phosphorene, is an emerging two-dimensional (2D) material, which has attracted increasing attention due to its unique electronic and optoelectronic properties. However, the reduced thermal stability of phosphorene limits its suitability for high-temperature fabrication processes, which could be detrimental for the performance of phosphorenebased devices. Here, we investigate the impact of doping by Al and Hf transition metal adatoms on the thermal stability of phosphorene. The formation of Al–P covalent bonds was found to significantly improve the thermal coefficients of the Ag1, B2g, and Ag2phonon modes to 0.00044, 0.00081, and 0.00012 cm–1·°C–1, respectively, which are two orders of magnitude lower than those observed for pristine P–P bonds (~0.01 cm–1·°C–1). First-principles calculations within the density functional theory framework reveal that the observed thermal stability enhancement in the Al-doped material reflects a significantly higher Al binding energy, due to the stronger Al–P bonds compared to the weak van der Waals interactions between adjacent P atoms in the undoped material. The present work thus paves the way towards phosphorene materials with improved structural stability, which could be promising candidates for potential nanoelectronic and optoelectronic applications. [Figure not availab.e: see fulltext.] © 2016, Tsinghua University Press and Springer-Verlag Berlin Heidelberg.

关键词： phosphorene black phosphorus adatom doping transition metals thermal stability

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High-efficiency, broad-band and wide-angle optical absorption in ultra-thin organic photovoltaic devices

High-efficiency, broad-band and wide-angle optical absorptio...

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作者： Wang, Wenyan Hao, Yuying Cui, Yanxia Tian, Ximin Zhang, Ye Wang, Hua Shi, Fang Wei, Bin Huang, Wei Key Lab. of Advanced Transducers and Intelligent Control System Ministry of Education Taiyuan University of Technology Taiyuan 030024 China Key Laboratory of Interface Science and Engineering in Advanced Materials Taiyuan University of Technology Taiyuan 030024 China Key Laboratory of Advanced Display and System Applications Ministry of Education Shanghai University Yanchang Road 149 Shanghai 200072 China Nanjing 210046 China

Metal nanogratings as one of the promising architectures for effective light trapping in organic photovoltaics (OPVs) have been actively studied over the past decade. Here we designed a novel metal nanowall grating with ultra-small period and ultra-high aspect-ratio as the back electrode of the OPV device. Such grating results in the strong hot spot effect in-between the neighboring nanowalls and the localized surface plasmon effect at the corners of nanowalls. These combined effects make the integrated absorption efficiency of light over the wavelength range from 400 to 650 nm in the active layer for the proposed structure, with respect to the equivalent planar structure, increases by 102% at TM polarization and by 36.5% at the TM/TE hybrid polarization, respectively. Moreover, it is noted that the hot spot effect in the proposed structure is more effective for ultra-thin active layers, which is very favorable for the exciton dissociation and charge collection. Therefore such a nanowall grating is expected to improve the overall performance of OPV devices. © 2014 Optical Society of America.

关键词： Light absorption

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Investigation on hole mobility of FeCl3-doped 4, 4'-bis(carbazol-9-yl) -biphenyl by using space-charge-limited current model

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Guangdianzi Jiguang/Journal of Optoelectronics Laser 2014年第7期25卷 1288-1293页

作者： Yuan, Shu-Qing Zhu, Yuan-Li Wang, Zhen-Guo Hao, Yu-Ying Wang, Hua Xu, Bing-She Key Laboratory of Advanced Transducers and Intelligent Control System College of Physics and Optoelectronics Taiyuan University of Technology Taiyuan 030024 China Key Lab of Interface Science and Engineering in Advanced Materials of Education Ministry of China Taiyuan University of Technology Taiyuan 030024 China

A series of single hole devices are designed based on the different concentrations of FeCl3 doped in 4, 4'-Bis(9H-carbazol-9-yl)biphenyl (CBP). The hole mobilities of p-type doped CBP by FeCl3 with various doping concentrations are estimated by using space-charge-limited current model, and compared with the mobility of NPB which is a kind of hole transport material commonly used in organic electroluminescence devices. The results indicate that FeCl3 doped CBP has significantly improved hole mobility. The highest hole mobility is achieved when the concentration of FeCl3 is 12%. For an electric field of 0.5 MV/cm, the estimated hole mobility of FeCl3-doped CBP with doping concentration of 12% reaches 4.5×10-5 cm2/V · s. Even in zero electric field, the hole mobility can reach 2.2×10-5 cm2/V · s, which is nearly four times of that of NPB. High efficiency organic light-emitting device is fabricated by using CBP: 12% FeCl3 as the hole transport layer. The device shows a maximum luminance of 68468 cd/m2 and a maximum current efficiency of 31.1 cd/A, which are increased by 97% and 23% compared with those of the reference device, respectively. The improvements are attributed to the balanced charge carrier transport characteristic, which results in an increased charge carrier recombination probability and a decreased triplet-polaron (T-P) annihilation probability.

关键词： Hole mobility

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Investigation on electroluminescence spectra regulation of OLEDs based on Zn(4-TfmBTZ)2

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Guangdianzi Jiguang/Journal of Optoelectronics Laser 2013年第5期24卷 892-896页

作者： Yan, Zheng-Fu Li, Yun-Fei Wang, Wen-Yan Hao, Yu-Ying Wang, Hua Xu, Bing-She College of Physics and Optoelectronics Taiyuan University of Technology Taiyuan 030024 China Key Lab. of Interface Science and Engineering in Advanced Materials of Education Ministry of China Taiyuan University of Technology Taiyuan 030024 China

The doping devices with structure of ITO/NPB/mcp:Zn(4-TfmBTZ)2/Bphen/LiF/Al are fabricated, where the Zn(4-TfmBTZ)2 mass fraction in mcp layer is 8% and 50%, respectively. The results show that the mass fraction of Zn(4-TfmBTZ)2 in mcp layer has important effect on the device performance, which contains spectrum and chromaticity. When the Zn(4-TfmBTZ)2 mass fraction is 8%, there exists a strong exciplex emission of Zn(4-TfmBTZ)2 and Bphen, while when the Zn(4-TfmBTZ)2 mass fraction is enhanced to 50%, the exciplex emission almost disappears. The light color is tuned from blue light CIEx,y(0.22, 0.27)to white light CIEx,y(0.29, 0.34) at the same voltage by changing the Zn(4-TfmBTZ)2 doping amount in mcp layer.

关键词： Light

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